WO2015152737A2 - Doped rare earth nitride materials and devices comprising same - Google Patents
Doped rare earth nitride materials and devices comprising same Download PDFInfo
- Publication number
- WO2015152737A2 WO2015152737A2 PCT/NZ2015/050039 NZ2015050039W WO2015152737A2 WO 2015152737 A2 WO2015152737 A2 WO 2015152737A2 NZ 2015050039 W NZ2015050039 W NZ 2015050039W WO 2015152737 A2 WO2015152737 A2 WO 2015152737A2
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- WIPO (PCT)
- Prior art keywords
- rare earth
- magnesium
- earth nitride
- nitride material
- doped rare
- Prior art date
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- 229910052761 rare earth metal Inorganic materials 0.000 title claims abstract description 337
- -1 rare earth nitride Chemical class 0.000 title claims abstract description 316
- 239000000463 material Substances 0.000 title claims abstract description 240
- 238000000034 method Methods 0.000 claims abstract description 119
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 89
- FLATXDRVRRDFBZ-UHFFFAOYSA-N azanylidynegadolinium Chemical compound [Gd]#N FLATXDRVRRDFBZ-UHFFFAOYSA-N 0.000 claims description 85
- 239000011777 magnesium Substances 0.000 claims description 47
- SZZXSKFKZJTWOY-UHFFFAOYSA-N azanylidynesamarium Chemical compound [Sm]#N SZZXSKFKZJTWOY-UHFFFAOYSA-N 0.000 claims description 44
- IBIOTXDDKRNYMC-UHFFFAOYSA-N azanylidynedysprosium Chemical compound [Dy]#N IBIOTXDDKRNYMC-UHFFFAOYSA-N 0.000 claims description 43
- VZVZYLVXLCEAMR-UHFFFAOYSA-N azanylidyneerbium Chemical compound [Er]#N VZVZYLVXLCEAMR-UHFFFAOYSA-N 0.000 claims description 43
- YKIJUSDIPBWHAH-UHFFFAOYSA-N azanylidyneholmium Chemical compound [Ho]#N YKIJUSDIPBWHAH-UHFFFAOYSA-N 0.000 claims description 43
- OVMJQLNJCSIJCH-UHFFFAOYSA-N azanylidyneneodymium Chemical compound [Nd]#N OVMJQLNJCSIJCH-UHFFFAOYSA-N 0.000 claims description 43
- 229910045601 alloy Inorganic materials 0.000 claims description 42
- 239000000956 alloy Substances 0.000 claims description 42
- 229910052757 nitrogen Inorganic materials 0.000 claims description 42
- 229910052749 magnesium Inorganic materials 0.000 claims description 39
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 claims description 37
- 239000000758 substrate Substances 0.000 claims description 37
- DPDGELPGCPPHSN-UHFFFAOYSA-N azanylidynelutetium Chemical compound [Lu]#N DPDGELPGCPPHSN-UHFFFAOYSA-N 0.000 claims description 25
- QCLQZCOGUCNIOC-UHFFFAOYSA-N azanylidynelanthanum Chemical compound [La]#N QCLQZCOGUCNIOC-UHFFFAOYSA-N 0.000 claims description 24
- PSBUJOCDKOWAGJ-UHFFFAOYSA-N azanylidyneeuropium Chemical compound [Eu]#N PSBUJOCDKOWAGJ-UHFFFAOYSA-N 0.000 claims description 23
- JCWZBEIBQMTAIH-UHFFFAOYSA-N azanylidynepraseodymium Chemical compound [Pr]#N JCWZBEIBQMTAIH-UHFFFAOYSA-N 0.000 claims description 23
- DOHQPUDBULHKAI-UHFFFAOYSA-N azanylidyneterbium Chemical compound [Tb]#N DOHQPUDBULHKAI-UHFFFAOYSA-N 0.000 claims description 23
- PTXUCVLZGJKEFB-UHFFFAOYSA-N azanylidynethulium Chemical compound [Tm]#N PTXUCVLZGJKEFB-UHFFFAOYSA-N 0.000 claims description 23
- XLWMYKCPNRBIDK-UHFFFAOYSA-N azanylidyneytterbium Chemical compound [Yb]#N XLWMYKCPNRBIDK-UHFFFAOYSA-N 0.000 claims description 23
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims description 19
- 150000002910 rare earth metals Chemical class 0.000 claims description 18
- 239000010408 film Substances 0.000 claims description 16
- 239000002019 doping agent Substances 0.000 claims description 15
- 238000000151 deposition Methods 0.000 claims description 14
- 238000001451 molecular beam epitaxy Methods 0.000 claims description 13
- 230000005294 ferromagnetic effect Effects 0.000 claims description 11
- 239000010409 thin film Substances 0.000 claims description 10
- 229910052688 Gadolinium Inorganic materials 0.000 claims description 9
- 229910021529 ammonia Inorganic materials 0.000 claims description 8
- 230000004907 flux Effects 0.000 claims description 8
- 238000005259 measurement Methods 0.000 claims description 8
- 238000004549 pulsed laser deposition Methods 0.000 claims description 8
- 229910052692 Dysprosium Inorganic materials 0.000 claims description 7
- 229910052689 Holmium Inorganic materials 0.000 claims description 7
- 239000012535 impurity Substances 0.000 claims description 7
- 238000005240 physical vapour deposition Methods 0.000 claims description 6
- 238000001755 magnetron sputter deposition Methods 0.000 claims description 4
- 239000000203 mixture Substances 0.000 claims description 3
- 238000002207 thermal evaporation Methods 0.000 claims description 3
- 238000004519 manufacturing process Methods 0.000 abstract description 5
- 230000005693 optoelectronics Effects 0.000 abstract description 4
- 125000004429 atom Chemical group 0.000 description 19
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 7
- 230000005291 magnetic effect Effects 0.000 description 7
- 150000004767 nitrides Chemical class 0.000 description 7
- 239000004065 semiconductor Substances 0.000 description 7
- 229910052710 silicon Inorganic materials 0.000 description 7
- 239000010703 silicon Substances 0.000 description 7
- 108091006149 Electron carriers Proteins 0.000 description 6
- 229910052733 gallium Inorganic materials 0.000 description 6
- 229910001199 N alloy Inorganic materials 0.000 description 4
- 238000002441 X-ray diffraction Methods 0.000 description 4
- 229910052782 aluminium Inorganic materials 0.000 description 4
- 230000008021 deposition Effects 0.000 description 4
- 229910052738 indium Inorganic materials 0.000 description 4
- 238000001004 secondary ion mass spectrometry Methods 0.000 description 4
- 239000007787 solid Substances 0.000 description 4
- 238000000354 decomposition reaction Methods 0.000 description 3
- 229910000069 nitrogen hydride Inorganic materials 0.000 description 3
- 230000003287 optical effect Effects 0.000 description 3
- 229910001218 Gallium arsenide Inorganic materials 0.000 description 2
- 229910019794 NbN Inorganic materials 0.000 description 2
- 229910052773 Promethium Inorganic materials 0.000 description 2
- 229910004166 TaN Inorganic materials 0.000 description 2
- 229910052804 chromium Inorganic materials 0.000 description 2
- 239000004020 conductor Substances 0.000 description 2
- 230000001419 dependent effect Effects 0.000 description 2
- 230000008020 evaporation Effects 0.000 description 2
- 238000001704 evaporation Methods 0.000 description 2
- 239000012212 insulator Substances 0.000 description 2
- 229910001635 magnesium fluoride Inorganic materials 0.000 description 2
- 238000001000 micrograph Methods 0.000 description 2
- VQMWBBYLQSCNPO-UHFFFAOYSA-N promethium atom Chemical compound [Pm] VQMWBBYLQSCNPO-UHFFFAOYSA-N 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 229910052721 tungsten Inorganic materials 0.000 description 2
- 229910001233 yttria-stabilized zirconia Inorganic materials 0.000 description 2
- 229910052684 Cerium Inorganic materials 0.000 description 1
- 229910052691 Erbium Inorganic materials 0.000 description 1
- 229910052693 Europium Inorganic materials 0.000 description 1
- 229910002601 GaN Inorganic materials 0.000 description 1
- 230000005355 Hall effect Effects 0.000 description 1
- 229910052765 Lutetium Inorganic materials 0.000 description 1
- 229910052779 Neodymium Inorganic materials 0.000 description 1
- 229910052777 Praseodymium Inorganic materials 0.000 description 1
- 229910052772 Samarium Inorganic materials 0.000 description 1
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical group [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 description 1
- 229910052771 Terbium Inorganic materials 0.000 description 1
- 229910052775 Thulium Inorganic materials 0.000 description 1
- 229910052769 Ytterbium Inorganic materials 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- GWXLDORMOJMVQZ-UHFFFAOYSA-N cerium Chemical compound [Ce] GWXLDORMOJMVQZ-UHFFFAOYSA-N 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 230000000295 complement effect Effects 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 238000006731 degradation reaction Methods 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000018109 developmental process Effects 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- KBQHZAAAGSGFKK-UHFFFAOYSA-N dysprosium atom Chemical compound [Dy] KBQHZAAAGSGFKK-UHFFFAOYSA-N 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- UYAHIZSMUZPPFV-UHFFFAOYSA-N erbium Chemical compound [Er] UYAHIZSMUZPPFV-UHFFFAOYSA-N 0.000 description 1
- OGPBJKLSAFTDLK-UHFFFAOYSA-N europium atom Chemical compound [Eu] OGPBJKLSAFTDLK-UHFFFAOYSA-N 0.000 description 1
- 239000003302 ferromagnetic material Substances 0.000 description 1
- 230000005669 field effect Effects 0.000 description 1
- UIWYJDYFSGRHKR-UHFFFAOYSA-N gadolinium atom Chemical compound [Gd] UIWYJDYFSGRHKR-UHFFFAOYSA-N 0.000 description 1
- RJOJUSXNYCILHH-UHFFFAOYSA-N gadolinium(3+) Chemical compound [Gd+3] RJOJUSXNYCILHH-UHFFFAOYSA-N 0.000 description 1
- KJZYNXUDTRRSPN-UHFFFAOYSA-N holmium atom Chemical compound [Ho] KJZYNXUDTRRSPN-UHFFFAOYSA-N 0.000 description 1
- 238000002513 implantation Methods 0.000 description 1
- 229910052746 lanthanum Inorganic materials 0.000 description 1
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 description 1
- OHSVLFRHMCKCQY-UHFFFAOYSA-N lutetium atom Chemical compound [Lu] OHSVLFRHMCKCQY-UHFFFAOYSA-N 0.000 description 1
- 230000005415 magnetization Effects 0.000 description 1
- 238000002488 metal-organic chemical vapour deposition Methods 0.000 description 1
- 238000012544 monitoring process Methods 0.000 description 1
- QEFYFXOXNSNQGX-UHFFFAOYSA-N neodymium atom Chemical compound [Nd] QEFYFXOXNSNQGX-UHFFFAOYSA-N 0.000 description 1
- 125000004433 nitrogen atom Chemical group N* 0.000 description 1
- 239000002674 ointment Substances 0.000 description 1
- PUDIUYLPXJFUGB-UHFFFAOYSA-N praseodymium atom Chemical compound [Pr] PUDIUYLPXJFUGB-UHFFFAOYSA-N 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 238000002128 reflection high energy electron diffraction Methods 0.000 description 1
- KZUNJOHGWZRPMI-UHFFFAOYSA-N samarium atom Chemical compound [Sm] KZUNJOHGWZRPMI-UHFFFAOYSA-N 0.000 description 1
- GZCRRIHWUXGPOV-UHFFFAOYSA-N terbium atom Chemical compound [Tb] GZCRRIHWUXGPOV-UHFFFAOYSA-N 0.000 description 1
- FRNOGLGSGLTDKL-UHFFFAOYSA-N thulium atom Chemical compound [Tm] FRNOGLGSGLTDKL-UHFFFAOYSA-N 0.000 description 1
- NAWDYIZEMPQZHO-UHFFFAOYSA-N ytterbium Chemical compound [Yb] NAWDYIZEMPQZHO-UHFFFAOYSA-N 0.000 description 1
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- C30B23/00—Single-crystal growth by condensing evaporated or sublimed materials
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- C30B23/06—Heating of the deposition chamber, the substrate or the materials to be evaporated
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- H01L21/02518—Deposited layers
- H01L21/0257—Doping during depositing
- H01L21/02573—Conductivity type
- H01L21/02576—N-type
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- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L21/00—Processes or apparatus adapted for the manufacture or treatment of semiconductor or solid state devices or of parts thereof
- H01L21/02—Manufacture or treatment of semiconductor devices or of parts thereof
- H01L21/02104—Forming layers
- H01L21/02365—Forming inorganic semiconducting materials on a substrate
- H01L21/02518—Deposited layers
- H01L21/0257—Doping during depositing
- H01L21/02573—Conductivity type
- H01L21/02579—P-type
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- H—ELECTRICITY
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- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L21/00—Processes or apparatus adapted for the manufacture or treatment of semiconductor or solid state devices or of parts thereof
- H01L21/02—Manufacture or treatment of semiconductor devices or of parts thereof
- H01L21/02104—Forming layers
- H01L21/02365—Forming inorganic semiconducting materials on a substrate
- H01L21/02612—Formation types
- H01L21/02617—Deposition types
- H01L21/02631—Physical deposition at reduced pressure, e.g. MBE, sputtering, evaporation
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- H01L29/02—Semiconductor bodies ; Multistep manufacturing processes therefor
- H01L29/12—Semiconductor bodies ; Multistep manufacturing processes therefor characterised by the materials of which they are formed
- H01L29/24—Semiconductor bodies ; Multistep manufacturing processes therefor characterised by the materials of which they are formed including, apart from doping materials or other impurities, only semiconductor materials not provided for in groups H01L29/16, H01L29/18, H01L29/20, H01L29/22
Definitions
- the present invention relates to rare earth nitride semiconductors and, more particularly, to magnesium-doped rare earth nitride materials, some of which are semi-insulating or insulating.
- the present invention further relates to methods for preparing the materials, and devices comprising the materials.
- the rare earths have atomic numbers from 57 (La) to 71 (Lu), and comprise the elements across which the 4f orbitals are filled: that is, lanthanum (La), cerium (Ce), praseodymium (Pr), neodymium (Nd), promethium (Pm), samarium (Sm), europium (Eu), gadolinium (Gd), terbium (Tb), dysprosium (Dy), holmium (Ho), erbium (Er), thulium (Tm), ytterbium (Yb), and lutetium (Lu).
- La lanthanum
- Ce cerium
- Pr praseodymium
- Nd neodymium
- Pm promethium
- Sm samarium
- Eu europium
- Gd gadolinium
- Tb terbium
- Dy dysprosium
- Ho holmium
- Er erbium
- the rare earth nitrides form in the face-centered cubic NaCl structure with lattice constants ranging from -5.3 A for LaN to -4.76 A for LuN, in total a 10% difference across the series and about 0.7% between nitrides of neighbouring atomic species.
- the rare earth nitrides were first investigated in the 1960s, when technological developments overcame the problems faced in separating the chemically similar members of the rare earth series.
- the rare earth nitrides have interesting magnetic and electronic properties.
- the rare earth nitrides have an optical bandgap typically of the order of 1 eV and are almost all ferromagnetic, with magnetic states that vary strongly across the series and coercive fields depending strongly on the growth conditions.
- SmN is the only known near-zero-moment ferromagnetic semiconductor, with an enormous coercive field, and GdN has a coercive field some three orders of magnitude smaller.
- the rare earth nitrides show promise in applications as diverse as spintronics, infrared (IR) detectors, and as contacts to group III nitride semiconductor compounds.
- rare earth nitrides have been used in the fabrication of spin-filter Josephson junctions and field effect transistor structures.
- the rare earth nitrides are also epitaxy-compatible materials with group III nitride
- GaN tunnel junctions a technologically important family of materials for the fabrication of, for example, optoelectronic devices and high power transistors.
- the properties of the rare earth nitrides are also complementary with those of the group III nitrides.
- a heteroj unction involving these two semiconductor materials could have very attractive properties for multi-wavelength photonic devices and spin light emitting diodes.
- GdN quantum dots have been shown to enhance the efficiency of GaN tunnel junctions.
- Semi-insulating and insulating rare earth nitride layers could be useful, optionally in combination with group III nitrides, in the fabrication of, for example, spintronics, electronic and optoelectronic devices. Such layers may avoid, for example, leakage current or degradation of radio frequency performance of such devices.
- High quality epitaxial thin films of rare earth nitrides can be grown using ultra-high vacuum (UHV)-based methods, such as molecular beam epitaxy (MBE), pulsed-laser deposition (PLD), and DC/RF magnetron sputtering.
- UHV-based methods typically result in unintentionally doped films that have a resistivity of the order of 0.05 to 10 mQ.cm at room temperature and an n-type residual doping concentration associated with a background electron carrier concentration ranging from 10 to 10 cm , which originates from nitrogen vacancy and depends on the growth conditions.
- the present invention provides a magnesium-doped rare earth nitride material, wherein the rare earth nitride is selected from the group consisting of lanthanum nitride (LaN), praseodymium nitride (PrN), neodymium nitride (NdN), samarium nitride (SmN), europium nitride (EuN), gadolinium nitride (GdN), terbium nitride (TbN), dysprosium nitride (DyN), holmium nitride (HoN), erbium nitride (ErN), thulium nitride (TmN), ytterbium nitride (YbN), and lutetium nitride (LuN), and alloys of any two or more thereof.
- the present invention provides a method of lanthanum nitride (
- the present invention provides a magnesium-doped rare earth nitride material when prepared by a method of the second aspect.
- the present invention also provides a magnesium-doped rare earth nitride material obtainable by a method of the second aspect.
- the present invention also provides a device comprising a magnesium-doped rare earth nitride material of the invention.
- This invention may also be said broadly to consist in the parts, elements and features referred to or indicated in the specification of the application, individually or collectively, and any or all combinations of any two or more said parts, elements or features, and where specific integers are mentioned herein which have known equivalents in the art to which this invention relates, such known equivalents are deemed to be incorporated herein as if individually set forth.
- features or aspects of the invention are described in terms of Markush groups, those persons skilled in the art will appreciate that the invention is also thereby described in terms of any individual member or subgroup of members of the Markush group.
- magnesium-doped rare earth nitride material has a resistivity between about 10 3 Q.cm and about 1010 Q.cm at room temperature.
- insulating means that the magnesium-doped rare earth nitride material has a resistivity greater than about 10 10 Q.cm at room temperature.
- Figure 1 is a cross section scanning electron microscope image showing the structure of a layer of Mg-doped GdN on a substrate, which comprises an AIN buffer layer deposited on silicon, and with a GaN capping layer;
- Figure 2 shows the (1 1 1) x-ray rocking curves for a Mg-doped GdN layer and for an undoped GdN layer
- Figure 3 shows the measured secondary ion mass spectrometry magnesium profile of a Mg- doped GdN layer on a substrate, which comprises an A1N buffer layer deposited on silicon, and with a GaN capping layer;
- Figure 4(a) shows the in-plane zero field-cooled magnetisation of a Mg-doped GdN layer
- Figure 4(b) shows the field-dependent magnetisation of a Mg-doped GdN layer
- Figure 5 shows the resistivity of Mg-doped GdN layers as a function of the electron carrier concentration.
- the present invention provides magnesium-doped rare earth nitride materials, some of which are semi-insulating and insulating.
- the present invention also provides a method for preparing such materials by doping the growing rare earth nitride materials with magnesium, which is an acceptor dopant species, to compensate for the donor species and increase the resistivity.
- the method of the invention enables control of the conductivity of the rare earth nitride materials from n-type through to semi-insulating and insulating.
- the present invention provides a magnesium-doped rare earth nitride material, wherein the rare earth nitride is selected from the group consisting of lanthanum nitride (LaN), praseodymium nitride (PrN), neodymium nitride (NdN), samarium nitride (SmN), europium nitride (EuN), gadolinium nitride (GdN), terbium nitride (TbN), dysprosium nitride (DyN), holmium nitride (HoN), erbium nitride (ErN), thulium nitride (TmN), ytterbium nitride (YbN), and lutetium nitride (LuN), and alloys of any two or more thereof.
- LaN lanthanum nitride
- PrN prase
- the present invention also provides a magnesium-doped rare earth nitride material, wherein the rare earth nitride is selected from the group consisting of LaN, PrN, NdN, SmN, EuN, GdN, TbN, DyN, HoN, ErN, TmN, YbN, and LuN, and alloys of any two or more thereof, and wherein the magnesium-doped rare earth nitride material has an increased resistivity compared to the undoped rare earth nitride material.
- the present invention also provides a semi-insulating or insulating magnesium-doped rare earth nitride material, wherein the rare earth nitride is selected from the group consisting of LaN, PrN, NdN, SmN, EuN, GdN, TbN, DyN, HoN, ErN, TmN, YbN, and LuN, and alloys of any two or more thereof.
- the present invention also provides a magnesium-doped rare earth nitride material having a resistivity of at least about 25 Q.cm, wherein the rare earth nitride is selected from the group consisting of LaN, PrN, NdN, SmN, EuN, GdN, TbN, DyN, HoN, ErN, TmN, YbN, and LuN, and alloys of any two or more thereof.
- the present invention also provides a magnesium-doped rare earth nitride material having a resistivity of at least about 10 ⁇ . ⁇ , wherein the rare earth nitride is selected from the group consisting of LaN, PrN, NdN, SmN, EuN, GdN, TbN, DyN, HoN, ErN, TmN, YbN, and LuN, and alloys of any two or more thereof.
- the present invention also provides a magnesium-doped rare earth nitride material having a resistivity between about 10 3 Q.cm and about 101 ⁇ 0 ⁇ ⁇ .cm, wherein the rare earth nitride is selected from the group consisting of LaN, PrN, NdN, SmN, EuN, GdN, TbN, DyN, HoN, ErN, TmN, YbN, and LuN, and alloys of any two or more thereof.
- the present invention also provides a magnesium-doped rare earth nitride material having a resistivity of at least about 10 10 Q.cm, wherein the rare earth nitride is selected from the group consisting of LaN, PrN, NdN, SmN, EuN, GdN, TbN, DyN, HoN, ErN, TmN, YbN, and LuN, and alloys of any two or more thereof.
- the magnesium-doped rare earth nitride material of the invention has a resistivity of at least about 5x 10 ⁇ . ⁇ . In some embodiments, the magnesium-doped rare earth nitride material of the invention has a resistivity of at least about 10 4 ⁇ . ⁇ .
- undoped GdN typically has a resistivity of about 2x 10 " ⁇ . ⁇ .
- the rare earth nitride is selected from the group consisting of LaN, PrN, NdN, SmN, EuN, GdN, TbN, DyN, HoN, ErN, TmN, YbN, and LuN. In some embodiments, the rare earth nitride is selected from the group consisting of LaN, PrN, NdN, SmN, GdN, TbN, DyN, HoN, ErN, TmN, and LuN, and alloys of any two or more thereof.
- the rare earth nitride is selected from the group consisting of LaN, PrN, NdN, SmN, GdN, TbN, DyN, HoN, ErN, TmN, and LuN. In some embodiments, the rare earth nitride is selected from the group consisting of NdN, SmN, EuN, GdN, DyN, HoN, ErN, and YbN, and alloys of any two or more thereof.
- the rare earth nitride is selected from the group consisting of NdN, SmN, EuN, GdN, DyN, HoN, ErN, and YbN.
- the rare earth nitride is selected from the group consisting of NdN, SmN, GdN, DyN, HoN, and ErN, and alloys of any two or more thereof.
- the rare earth nitride is selected from the group consisting of NdN, SmN, GdN, DyN, HoN, and ErN.
- the rare earth nitride is a rare earth nitride alloy.
- the rare earth nitride alloy is selected from the group consisting of (Sm,Gd)N, (Gd,Ho)N, and (Gd,Dy)N.
- the rare earth nitride alloy is (Sm,Gd)N.
- the rare earth nitride alloy is (Gd,Ho)N. In some embodiments, the rare earth nitride alloy is (Gd,Dy)N.
- the rare earth nitride is GdN.
- magnesium has been found to be effective to compensate residual donor species (that is, nitrogen vacancies) in rare earth nitrides and produce, in some embodiments, a rare earth nitride material that is at least semi-insulating.
- the magnesium-doped rare earth nitride material of the invention comprises about 10 18 -1021 1 atoms/cm 3" of magnesium. In some embodiments, the magnesium- doped rare earth nitride material of the invention comprises about 10 1 1 8 ⁇ -5 1020 ⁇ atoms/cm 3" of magnesium. In some embodiments, the magnesium-doped rare earth nitride material of the invention comprises about 10 19 -5x 1020 atoms/cm 3 of magnesium.
- the magnesium-doped rare earth nitride material of the invention may, however, further comprise one or more additional dopant(s).
- the magnesium-doped rare earth nitride material of the invention comprises less than about 1021 atoms/cm 3 of additional dopant(s) or other impurities.
- the magnesium-doped rare earth nitride material of the invention comprises less than about 10 20 atoms/cm 3 of additional dopant(s) or other impurities.
- the magnesium-doped rare earth nitride material of the invention comprises less than about 10 19 atoms/cm 3 of additional dopant(s) or other impurities.
- the magnesium-doped rare earth nitride material is a thin film.
- the film thickness is about 1 -2000 nm. In some embodiments, the film thickness is about 5-2000 nm. In some embodiments, the film thickness is about 1-1000 nm. In some embodiments, the film thickness is about 5-1000 nm. In some embodiments, the film thickness is about 10-200 nm.
- the magnesium-doped rare earth nitride material of the invention has an increased resistivity compared to the undoped rare earth nitride material.
- the magnetic properties of the magnesium-doped rare earth nitride material are, however, generally not substantially different to those of the undoped rare earth nitride material.
- the magnetic properties of the magnesium-doped rare earth nitride material can be measured using known techniques and instrumentation, such as a superconducting quantum interference device (SQUID).
- the magnesium-doped rare earth nitride material is ferromagnetic below about 50 , preferably below about 70 .
- the structural properties of the magnesium-doped rare earth nitride material are generally not substantially different to those of the undoped rare earth nitride material.
- the structural properties of the magnesium-doped rare earth nitride material can be measured using known techniques and instrumentation, such as x-ray diffraction (XRD) measurements.
- XRD x-ray diffraction
- the magnesium-doped rare earth nitride material has substantially the same XRD measurements as the undoped rare earth nitride.
- the magnesium-doped rare earth nitride material comprises a thin film on a substrate.
- Suitable substrates are non-reactive with the magnesium-doped rare earth nitride material and are stable during the processing conditions used for preparing the magnesium-doped rare earth nitride material.
- the substrate is a conductor.
- the substrate is a semiconductor.
- the substrate is an insulator.
- the substrate is crystalline, but the invention is not limited thereto.
- the magnesium-doped rare earth nitride material is epitaxial with the substrate. In other embodiments, the magnesium-doped rare earth nitride material is
- the substrate is AIN, GaN or an (Al,In,Ga)N alloy.
- suitable substrates include, but are not limited to, yttria-stabilized zirconia (YSZ) and MgO. Further suitable substrates include, but are not limited to Al, W, Cr, Cu, Gd, Mg, TaN, NbN, GaAs, and MgF 2 .
- Suitable substrates also include multilayer-structured materials.
- multilayer- structured substrates may comprise a buffer layer in contact with the magnesium-doped rare earth nitride material.
- the multilayer-structured material comprises a buffer layer of an undoped rare earth nitride.
- the substrate comprises Si or A1 2 0 3 , optionally with a buffer layer of AIN or GaN.
- the buffer layer is an (Al,In,Ga)N alloy.
- the substrate comprises deoxidized silicon oriented along the (1 1 1) plane. In some embodiments, the substrate comprises deoxidized silicon oriented along the (1 1 1) plane with an epitaxial AIN buffer layer.
- the magnesium-doped rare earth nitride material is capped.
- Suitable capping layers are non-reactive with the magnesium-doped rare earth nitride material.
- the capping layer may be epitaxial with the magnesium-doped rare earth nitride material, polycrystalline, or amorphous.
- the capping layer is a conductor. In other embodiments, the capping layer is a semiconductor. In other embodiments, the capping layer is an insulator.
- Suitable materials for the capping layer include, but are not limited to Al, W, Cr, Cu, Gd, Mg, TaN, NbN, Si, YSZ, GaN, GaAs, AIN, (Al,In,Ga)N alloys, and MgF 2 .
- the capping layer is selected from AIN, GaN, (Al,In,Ga)N alloys, and Si.
- the capping layer is selected from AIN and GaN.
- AIN and GaN are transparent, allowing optical measurements.
- Other advantages of AIN and GaN include their ease of growth and good chemical stability over time.
- the capping layer is GaN.
- the magnesium-doped rare earth nitride material may be prepared by growing the rare earth nitride in the presence of magnesium atoms.
- the invention is not limited thereto, and the magnesium-doped rare earth nitride material may be prepared by other methods known to those skilled in the art, including but not limited to implantation and diffusion methods.
- the present invention provides a method of preparing a magnesium-doped rare earth nitride material of the invention, the method comprising the step of:
- the magnesium-doped rare earth nitride material is deposited on a substrate. Suitable substrates are discussed above.
- the present invention provides a method of preparing a magnesium-doped rare earth nitride material of the invention, the method comprising the step of:
- the method further comprises the step of:
- step (b) depositing a capping layer on the magnesium-doped rare earth nitride deposited in step (a). Suitable capping layers are discussed above.
- the magnesium-doped rare earth nitride material, and the optional capping layer can be deposited using ultra-high vacuum techniques known to those skilled in the art. Suitable techniques include, but are not limited to, physical vapour deposition (PVD), including pulsed laser deposition (PLD) and DC/RF magnetron sputtering, thermal evaporation, and molecular beam epitaxy (MBE). Other techniques, including but not limited to metalorganic chemical vapour deposition (MOCVD), may also be used.
- PVD physical vapour deposition
- PLD pulsed laser deposition
- MBE molecular beam epitaxy
- MOCVD metalorganic chemical vapour deposition
- the magnesium-doped rare earth nitride material and the optional capping layer are sequentially deposited by MBE.
- reflection high energy electron diffraction (RHEED) is used for monitoring the growth of the layer(s).
- the base pressure in the MBE apparatus is typically about 10 " Torr or less.
- the magnesium source is a magnesium-containing substance capable of providing gaseous magnesium atoms at the growth surface.
- the magnesium source is magnesium.
- the magnesium source can be an effusion cell containing solid magnesium, which is evaporated during the deposition.
- the rare earth can be provided from a source of the rare earth element, such as an effusion cell containing the solid rare earth, which is evaporated during the deposition.
- a source of the rare earth element such as an effusion cell containing the solid rare earth, which is evaporated during the deposition.
- the nitrogen source provides reactive nitrogen atoms at the growth surface.
- the nitrogen source is selected from the group consisting of pure molecular nitrogen, ammonia, and a source of active nitrogen, such as a nitrogen plasma or ionized nitrogen, or mixtures of any two or more thereof.
- the nitrogen source is selected from the group consisting of pure molecular nitrogen, ammonia, and a source of active nitrogen, such as a nitrogen plasma or ionized nitrogen.
- the nitrogen source is ammonia.
- the nitrogen source flux is typically a factor of at least 100 larger than the rare earth flux. If the ratio of the nitrogen source flux to the rare earth flux is less than about 100, the resulting films are likely to be heavily doped by nitrogen vacancies.
- the partial pressure or beam equivalent pressure (BEP) of the nitrogen source is about 10 " 5 -10 "3 Torr, preferably about 10 "5 -10 "4 Torr.
- the BEP of the nitrogen source is about 1.9x l0 "5 Torr.
- the BEP of the rare earth is about 10 " -10 " Torr.
- the BEP of the rare earth is about 5x 10 " Torr.
- the BEP of magnesium is about 10 "9 -5> ⁇ 10 "6 Torr, preferably about 10 "9 - 5x l0 "7 Torr.
- the magnesium-doped rare earth nitride material is typically deposited at a rate of about 0.01-1 nm/second. In some embodiments, the magnesium-doped rare earth nitride material is deposited at a rate of about 0.01-0.5 nm/second. In some embodiments, the magnesium-doped rare earth nitride material is deposited at a rate of about 0.01-0.15 nm/second. In some embodiments, the magnesium-doped rare earth nitride material is deposited at a rate of about 0.01-0.1 nm/second.
- the magnesium-doped rare earth nitride material is deposited at ambient or elevated temperatures.
- the magnesium-doped rare earth nitride material is generally deposited at elevated temperatures where it is desirable that the material be epitaxial with the substrate on which it is to be deposited. Accordingly, in some embodiments, the magnesium-doped rare earth nitride material is deposited at a temperature of about 500-900 °C. In some embodiments, the magnesium-doped rare earth nitride material is deposited at a temperature of about 500-750 °C.
- the magnesium-doped rare earth nitride material may, however, be deposited at lower temperatures than those above, or even at ambient temperature, particularly if a polycrystalline material is desired. Depositing the magnesium-doped rare earth nitride material at lower temperatures typically results in fewer nitrogen vacancies.
- the temperature during the deposition may be conveniently measured with an optical pyrometer, or other suitable apparatus as is known in the art, for example a thermocouple.
- two or more rare earth elements are simultaneously evaporated in the presence of a nitrogen source and a magnesium source, as discussed above, to provide a magnesium-doped rare earth nitride material of the invention wherein the rare earth nitride is an alloy.
- the substrate and/or capping layer comprise(s) a group III nitride
- alloys of group III nitrides are also contemplated.
- one or more dopants may be introduced during deposition of the magnesium-doped rare earth nitride material. Such dopants can alter the magnetic and/or electric properties of the resulting magnesium-doped rare earth nitride material.
- the present invention provides a magnesium-doped rare earth nitride material when prepared by a method of the second aspect.
- the present invention also provides a magnesium-doped rare earth nitride material obtainable by a method of the second aspect.
- the magnesium-doped rare earth nitride material of the invention may be useful in the fabrication of, for example, spintronics, electronic and optoelectronic devices. Accordingly, the present invention also provides a device comprising a magnesium-doped rare earth nitride material of the invention.
- Gadolinium nitride films doped with magnesium were grown in a molecular beam epitaxy system equipped with conventional Al, Ga, Mg and Gd evaporation cells.
- the purity of the as-received Al, Ga, Mg and Gd solid charges was 6N5, 7N5, 5N and 3N, respectively.
- Atomic nitrogen species were produced by the thermally activated decomposition of ammonia (NH 3 ) on the growing surface. The purity of the NH 3 was 6N5.
- a 100 nm thick AIN buffer layer was grown on a deoxidized silicon substrate oriented along the (1 1 1) plane.
- BEP beam equivalent pressure
- the BEP of magnesium typically ranged from 10 "9 to 5x l0 "7 Torr.
- the thickness of the Mg-doped GdN films ranged from 100 nm to 200 nm.
- the Mg-doped GdN layers were capped with a 60 nm thick GaN layer to prevent decomposition in air.
- Undoped GdN films grown under the conditions described above had a resistivity of about 2x 10 " ⁇ -cm at room temperature, while incorporating Mg in the GdN layer led to higher resistivity.
- Mg-doped GdN layers with a Mg concentration of about l x 10 19 atoms/cm 3 and about 5x 10 19 atoms/cm 3 had resistivities of about 25 ⁇ . ⁇ and greater than 10 4 ⁇ . ⁇ , respectively.
- the resistivity was measured at room temperature using a van der Pauw geometry.
- the resistivity of undoped GdN films grown under the conditions described above is about 1.7x 10 " ⁇ . ⁇ at 4 .
- Figure 1 is a cross section scanning electron microscope image showing the structure of a 140 nm thick layer of Mg-doped GdN on a substrate, which comprises a 106 nm thick AIN buffer layer deposited on silicon, and with a 64 nm thick GaN capping layer.
- the crystalline order/quality of a Mg-doped GdN layer is comparable to that of an undoped GdN layer grown under the same conditions.
- Figure 2 shows that for a 140 nm thick Mg-doped GdN layer with a concentration of 5x 1019 Mg atoms/cm 3 grown at 650°C the (1 1 1) x-ray rocking curve full width at half maximum (FWHM) is comparable with the FWHM for an undoped GdN layer.
- Figure 3 shows the measured secondary ion mass spectrometry (SIMS) magnesium profile of a Mg-doped GdN layer on a substrate, which comprises an AIN buffer layer deposited on silicon, and with a GaN capping layer.
- the atomic concentration of magnesium is about l x lO 19 atoms/cm 3 .
- FIG. 4 The magnetization curves shown in Figure 4 confirm that the magnetic properties of a Mg-doped GdN layer are substantially the same as those of an undoped GdN layer.
- Figure 4(a) shows the in-plane zero field-cooled (ZFC) magnetisation under an applied field of 250 Oe of a 140 nm thick Mg-doped GdN layer with a Mg concentration of about 5 ⁇ 10 19 atoms/cm 3 measured by SIMS. The Curie temperature is about 70 as per undoped GdN thin films.
- Figure 4(b) shows the field-dependent magnetisation at 5 of a 140 nm thick Mg-doped GdN layer with a Mg
- FIG. 5 shows the resistivity of 100 nm thick Mg- doped GdN layers as a function of the electron carrier concentration.
- the room temperature resistivity varies inversely with the electron density over five orders of magnitude.
- an undoped GdN layer has a resistivity of about 0.002 Q.cm and an electron carrier
- a magnesium-doped rare earth nitride material wherein the rare earth nitride is selected from the group consisting of lanthanum nitride (LaN), praseodymium nitride (PrN), neodymium nitride (NdN), samarium nitride (SmN), europium nitride (EuN), gadolinium nitride (GdN), terbium nitride (TbN), dysprosium nitride (DyN), holmium nitride (HoN), erbium nitride (ErN), thulium nitride (TmN), ytterbium nitride (YbN), and lutetium nitride
- LaN lanthanum nitride
- PrN praseodymium nitride
- NdN neodymium n
- a method of preparing a magnesium-doped rare earth nitride material wherein the rare earth nitride is selected from the group consisting of lanthanum nitride (LaN),
- PrN praseodymium nitride
- NdN neodymium nitride
- SmN samarium nitride
- EuN europium nitride
- GdN gadolinium nitride
- TbN terbium nitride
- DyN dysprosium nitride
- HoN holmium nitride
- ErN erbium nitride
- TmN thulium nitride
- YbN ytterbium nitride
- LuN lutetium nitride
- magnesium-doped rare earth nitride material depositing the magnesium-doped rare earth nitride material.
- the rare earth nitride is selected from the group consisting of LaN, PrN, NdN, SmN, GdN, TbN, DyN, HoN, ErN, TmN, and LuN, and alloys of any two or more thereof.
- the rare earth nitride is selected from the group consisting of NdN, SmN, EuN, GdN, DyN, HoN, ErN, and YbN, and alloys of any two or more thereof.
- the rare earth nitride is selected from the group consisting of NdN, SmN, GdN, DyN, HoN, and ErN, and alloys of any two or more thereof.
- the rare earth nitride is selected from the group consisting of LaN, PrN, NdN, SmN, GdN, TbN, DyN, HoN, ErN, TmN, and LuN.
- the rare earth nitride is selected from the group consisting of NdN, SmN, EuN, GdN, DyN, HoN, ErN, and YbN.
- the rare earth nitride is selected from the group consisting of NdN, SmN, GdN, DyN, HoN, and ErN.
- the rare earth nitride is a rare earth nitride alloy.
- the rare earth nitride alloy is selected from the group consisting of (Sm,Gd)N, (Gd,Ho)N, and (Gd,Dy)N.
- the magnesium-doped rare earth nitride material comprises about 10 1 1 8 -lCr 21 atoms/cm 3" of magnesium.
- magnesium-doped rare earth nitride material further comprises one or more additional dopant(s).
- magnesium-doped rare earth nitride material comprises less than about 10 21 atoms/cm 3 of additional dopant(s) or other impurities.
- magnesium-doped rare earth nitride material depositing the magnesium-doped rare earth nitride material.
- step (b) depositing a capping layer on the magnesium-doped rare earth nitride deposited in step (a).
- a method of clause 55 wherein the ultra-high vacuum technique is selected from the group consisting of physical vapour deposition (PVD), pulsed laser deposition (PLD), DC/RF magnetron sputtering, thermal evaporation, and molecular beam epitaxy (MBE).
- PVD physical vapour deposition
- PLD pulsed laser deposition
- DC/RF magnetron sputtering thermal evaporation
- MBE molecular beam epitaxy
- the nitrogen source is selected from the group consisting of pure molecular nitrogen, ammonia, and a source of active nitrogen, or mixtures of any two or more thereof.
- a magnesium-doped rare earth nitride material when prepared by a method of clauses 29 to 69.
- a magnesium-doped rare earth nitride material obtainable by a method of clauses 29 to 69.
- a device comprising a magnesium-doped rare earth nitride material of clauses 1 to 28, 70 and 71.
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CN201580024829.8A CN106460229B (en) | 2014-04-02 | 2015-03-31 | Doped rare earth nitride materials and devices containing the same |
EP15772411.3A EP3127146A4 (en) | 2014-04-02 | 2015-03-31 | Doped rare earth nitride materials and devices comprising same |
US15/300,757 US10415153B2 (en) | 2014-04-02 | 2015-03-31 | Doped rare earth nitride materials and devices comprising same |
KR1020167030552A KR102328525B1 (en) | 2014-04-02 | 2015-03-31 | Doped rare earth nitride materials and devices comprising same |
JP2016560766A JP6618481B2 (en) | 2014-04-02 | 2015-03-31 | Doped rare earth nitride materials and devices containing the same |
NZ725495A NZ725495A (en) | 2014-04-02 | 2015-03-31 | Doped rare earth nitride materials and devices comprising same |
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- 2015-03-31 KR KR1020167030552A patent/KR102328525B1/en active IP Right Grant
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Cited By (6)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO2018104899A1 (en) | 2016-12-07 | 2018-06-14 | Victoria University Of Wellington | Rare earth nitride structures and devices and method for removing a passivating capping |
CN110073477A (en) * | 2016-12-07 | 2019-07-30 | 维多利亚联科有限公司 | For the rare earth nitride structure except depassivation cap, Apparatus and method for |
JP2020509573A (en) * | 2016-12-07 | 2020-03-26 | ビクトリア リンク リミテッド | Rare earth nitride structures and devices and methods for removing passivating capping |
US11217743B2 (en) | 2016-12-07 | 2022-01-04 | Victoria Link Limited | Rare earth nitride structures and devices and method for removing a passivating capping |
JP7131835B2 (en) | 2016-12-07 | 2022-09-06 | ビクトリア リンク リミテッド | Rare earth nitride structures and devices and method for removing passivation capping |
US10043871B1 (en) * | 2017-04-06 | 2018-08-07 | Ecole Polytechnique Federale De Lausanne (Epfl) | Rare earth nitride and group III-nitride structure or device |
Also Published As
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US20170022632A1 (en) | 2017-01-26 |
US10415153B2 (en) | 2019-09-17 |
KR20170005409A (en) | 2017-01-13 |
WO2015152737A3 (en) | 2016-01-14 |
NZ725495A (en) | 2020-05-29 |
JP6618481B2 (en) | 2019-12-11 |
KR102328525B1 (en) | 2021-11-19 |
CN106460229A (en) | 2017-02-22 |
JP2017511294A (en) | 2017-04-20 |
EP3127146A4 (en) | 2017-11-08 |
EP3127146A2 (en) | 2017-02-08 |
CN106460229B (en) | 2019-12-10 |
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